Somehow submerging the plants within a different medium to change the entire spectrum would also likely not achieve any gains either, because by doing that you can only reduce the total amount of energy in any part of the spectrum, not shift it elsewhere (afaik).
edit: added 'arbitrarily' - as replies point out, moving towards the lower-energy end of the spectrum is not hard.
Shifting frequency the other direction is much harder; some materials exist that can double the frequency of light (known as second harmonic generation), but it's not as cheap as fluorescence. They are used in green laser pointers to turn infrared light into green light.
Isn't this the entire principle behind using quantum dots in displays?
i.e. The quantum dots absorb light from the backlight and then re-emit it as a very specific color band.
What? Yes we do. It's called fluorescence.
If you find a color range not being used effectively, it's easy to drop the frequency down to a better one.